Carbon quantum dot-mediated Fe11 polyoxometalate enrichment for accelerated photocatalytic H2 evolution in a Zn0.5Cd0.5S system

doi:10.1016/S1872-2067(26)65071-1

Abstract

Abstract:

Photocatalytic hydrogen evolution represents a sustainable and promising avenue for clean energy generation through harnessing solar energy. This study presents a photocatalytic system Fe₁₁POM@CQD@Zn_0.5Cd_0.5S, designed to enhance photocatalytic hydrogen evolution while addressing persistent environmental challenges. This advanced composite synergistically integrates iron polyoxometalate Na₂₇[Fe₁₁(H₂O)₁₄(OH)₂(W₃O₁₀)₂(α-SbW₉O₃₃)₆] (Fe₁₁POM) with carbon quantum dots (CQD) and a zinc cadmium sulfide (Zn_0.5Cd_0.5S) matrix, optimizing charge separation and light absorption efficiency. This composite exhibits a remarkable hydrogen production rate of 32.18 mmol·g^-1·h^-1, accompanied by a turnover number of 32,394 and a turnover frequency of 10798 h^-1. Notably, the apparent quantum yield reaches approximately 40%, while the solar-to-hydrogen efficiency is measured at 1.69%. The synergistic integration of Fe₁₁POM, the CQD and Zn_0.5Cd_0.5S components optimizes charge separation and transfer, significantly enhancing photocatalytic activity. This innovative approach provides a promising strategy for developing high-performance photocatalysts for sustainable hydrogen production, offering insights into the design of efficient heterostructures to address crises of energy scarcity and environmental pollution as well as pave the way for future research in multifunctional photocatalytic systems.

Key words: Hydrogen evolution, Iron containing polyoxometalate, Trinary catalyst, Zn_0.5Cd_0.5S, Carbon quantum dots

Khalid Umer, Xiao Fang, Khuram Hasnain, Hira Shahid, Weize Sun, Chenyu Shi, Junhan Xie, Baochun Ma, Yong Ding. Carbon quantum dot-mediated Fe₁₁ polyoxometalate enrichment for accelerated photocatalytic H₂ evolution in a Zn_0.5Cd_0.5S system[J]. Chinese Journal of Catalysis, 2026, 88: 218-232.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65071-1

https://www.cjcatal.com/EN/Y2026/V88/I9/218

Figures/Tables 10

Fig. 1. (a) Schematic illustration of synthesis strategy. (b) Design of a three-component photocatalytic system.

Fig. 2. (a) FT-IR spectra of Fe11POM, CQD@Zn0.5Cd0.5S, and Fe11POM@CQD@Zn0.5Cd0.5S. (b) XRD plot of CQD, Zn0.5Cd0.5S and CQD@Zn0.5Cd0.5S, Fe11POM and Fe11POM@CQD@Zn0.5Cd0.5S. SEM images of Zn0.5Cd0.5S (c), CQD@Zn0.5Cd0.5S (d), and Fe11POM@CQD@Zn0.5Cd0.5S (e).

Fig. 3. (a) TEM image of Fe11POM@CQD@Zn0.5Cd0.5S. (b) HRTEM image of Fe11POM@CQD@Zn0.5Cd0.5S. (c-e) EDS mapping of the various elements present in Fe11POM@CQD@Zn0.5Cd0.5S.

Fig. 4. High resolution XPS spectra containing comparison of peaks in Zn0.5Cd0.5S and Fe11POM@CQD@Zn0.5Cd0.5S: Zn 2p (a); Cd 3d (b); S 2p (c). XPS spectrum comparison of peaks presented in Fe11POM and Fe11POM@CQD@Zn0.5Cd0.5S for region: Fe 2p (d); Sb 3d (e); W 4f (f).

Fig. 5. (a) Photocatalytic hydrogen evolution rate using CdS (1), Mn0.5Cd0.5S (2), Zn0.5Cd0.5S (3), MoS2 (4), Mn-MoS2 (5), Zn-MoS2 (6), SnS2 (7), Mn-SnS2 (8), and Zn-SnS2 (9) catalysts. (b) Photocatalytic hydrogen evolution activity by attaching Fe11POM with catalysts CdS, Mn0.5Cd0.5S, Zn0.5Cd0.5S, MoS2, Mn-MoS2, Zn-MoS2, SnS2, Mn-SnS2 and Zn-SnS2. (c) Photocatalytic hydrogen evolution activity of CQD@CdS, CQD@Mn0.5Cd0.5S, CQD@Zn0.5Cd0.5S, CQD@MoS2, CQD@Mn-MoS2, CQD@Zn-MoS2, CQD@SnS2, CQD@Mn-SnS2 and CQD@Zn-SnS2. (d,e) Photocatalytic hydrogen evolution activity of Fe11POM@CQD@Zn0.5Cd0.5S, Fe11POM@Zn0.5Cd0.5S, CQD@Zn0.5Cd0.5S and Zn0.5Cd0.5S. (f) Durability test for composite photocatalyst material Fe11POM@CQD@Zn0.5Cd0.5S under same reaction conditions. (g) Comparison of AQY for H2 evolution of reported POM based catalysts with Fe11POM@CQD@Zn0.5Cd0.5S. Reaction conditions: 29 mL reactor, 5 mg of catalyst, 15 mL of aqueous lactic acid solution (10%, v/v), light source 420 nm LED lamp (100 mW·cm-2).

Fig. 6. (a) FT-IR spectra and (b) XRD patterns of fresh and used Fe11POM@CQD@Zn0.5Cd0.5S catalyst. XPS analysis of Fe11POM@CQD@Zn0.5Cd0.5S catalyst in its fresh and used states for Fe 2p (c), W 4f (d), Cd 3d (e), Zn 2p (f), S 2p (g), O 1s (h), and C 1s (i).

Fig. 7. (a) UV-vis DRS measurements of Fe11POM@CQD@Zn0.5Cd0.5S, CQD@Zn0.5Cd0.5S, Zn0.5Cd0.5S, Fe11POM, and CQD. (b) Tauc plots of Zn0.5Cd0.5S. (c) Mott-Schottky plot of Zn0.5Cd0.5S and Fe11POM. (d) VB-XPS of Fe11POM.

Fig. 8. (a) The transient i-t curves, (b) EIS plots and (c) PL emission spectra of Zn0.5Cd0.5S, Fe11POM and Fe11POM@CQD@Zn0.5Cd0.5S. (d) TRPLS of Zn0.5Cd0.5S and Fe11POM@CQD@Zn0.5Cd0.5S.

Fig. 9. (a-d) KPFM images of Fe11POM, Zn0.5Cd0.5S, CQD@Zn0.5Cd0.5S, and Fe11POM@CQD@Zn0.5Cd0.5S. (e-h) KPFM potential images of Fe11POM, Zn0.5Cd0.5S, CQD@Zn0.5Cd0.5S and Fe11POM@CQD@Zn0.5Cd0.5S under dark conditions. (i-l) KPFM images of Fe11POM, Zn0.5Cd0.5S, CQD@Zn0.5Cd0.5S and Fe11POM@CQD@Zn0.5Cd0.5S under light conditions. (m-p) Surface potential distribution diagrams across Fe11POM, Zn0.5Cd0.5S, CQD@Zn0.5Cd0.5S and Fe11POM@CQD@Zn0.5Cd0.5S before and after illumination.

Fig. 10. Possible reaction mechanism of photocatalytic hydrogen evolution reaction using Fe11POM@CQD@Zn0.5Cd0.5S system.

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Carbon quantum dot-mediated Fe₁₁ polyoxometalate enrichment for accelerated photocatalytic H₂ evolution in a Zn_0.5Cd_0.5S system

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